Journal Article Enhancement in Kinetics of the Oxygen Reduction Reaction on a Nitrogen-Doped Carbon Catalyst by Introduction of Iron via Electrochemical Methods

張, 達  ,  unknown, unknown  ,  尾嶋, 正治  ,  Oshima, Masaharu  ,  難波江, 裕太  ,  Nabae, Yuta  ,  岡島, 武義  ,  OKAJIMA, TAKEYOSHI  ,  大坂, 武男  ,  OHSAKA, TAKEO

31 ( No. 19 )  , pp.5529 - 5536 , 2015-04 , American Chemical Society
The iron (Fe) electrodeposition?electrochemical dissolution has been employed on nitrogen-doped carbon material (P-PI) prepared via multi-step pyrolysis of a polyimide precursor to achieve the introduction of Fe species, and its influence on the oxygen reduction reaction (ORR) is investigated by cyclic and rotating ring-disk electrode voltammetry in 0.5 M H2SO4. After the electrochemical treatment, the overpotential and H2O2 production percentage of ORR on the P-PI are decreased and the number of electrons transferred is increased in the meanwhile. In combination with the results of X-ray absorption fine structure spectra, the presence of Fe?Nx sites (Fe ions coordinated by nitrogen) is believed to be responsible for the improved ORR performance. Further kinetic analysis indicates that a two-electron reduction of O2 is predominant on the untreated P-PI with coexistence of a direct four-electron transformation of O2 to H2O, while the introduction of Fe species leads to a larger increase in the rate constant for the four-electron reduction than that for the two-electron process, being in good agreement with the view that Fe?Nx sites are active for four-electron ORR.

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